Abstract:
After doping different transition metals into metal-organic framework compounds, transition metal modified nitrogen-doped porous carbon material(M@NHC) was obtained by high temperature calcination. Then, Pt/M@NHC catalyst was prepared by colloidal deposition method and evaluated for catalytic oxidation of glycerol to glyceric acid under alkaline conditions. The result showed that the types of transition metals had a great influence on the conversion of glycerol and the glyceric acid selectivity, and the Ni-doped Pt/Ni@NHC catalyst exhibited the best catalytic activity. Combined with the characterization results of N
2 physical adsorption, X-ray diffraction, X-ray photoelectron spectroscopy, and CO
2 temperature programmed desorption, it was found that the introduction of Ni not only changed the surface electronic structure of Pt, but also increased the antioxidant capacity of Pt nanoparticles
via Ni-Pt synergies between metals. At the same time, the doping of surface nitrogen atoms increased the electrons on the Pt and adsorption oxygen surfaces, which would rapidly activate molecular oxygen and produce more active sites. In addition, Pt nanoparticles of Pt/Ni@NHC had the smallest particle size in all catalysts, which was conducive to the improvement of catalytic performance. The catalytic performance of Pt/Ni@NHC catalysts under different preparation conditions was investigated. The catalyst of Pt/Ni@NHC prepared under the conditions of 3% Ni content, calcination temperature of 800 ℃, the reaction pressure of 1 MPa and the reaction time of 6 h had the best catalytic performance. At this time, the conversion rate of glycerol was 63% and the selectivity of glyceric acid was 77.4%.